Abstract. The aerosol impact on liquid water path (LWP) is a key uncertainty in the overall climate impact of aerosol. However, despite a significant effort in this area, the size of the effect remains poorly constrained, and even the sign is unclear. Recent studies have shown that the relationship between droplet number concentration (Nd) and LWP is an unreliable measure of the impact of Nd variations on LWP due to the difficulty in establishing causality. In this work, we use satellite observations of the short-term development of clouds to examine the role of Nd perturbations in LWP variations. Similar to previous studies, an increase followed by a general decrease in LWP with increasing Nd is observed, suggesting an overall negative LWP response to Nd and a warming LWP adjustment to aerosol. However, the Nd also responds to the local environment, with aerosol production, entrainment from the free troposphere and wet scavenging all acting to modify the Nd. Many of these effects act to further steepen the Nd–LWP relationship and obscure the causal Nd impact on LWP. Using the temporal development of clouds to account for these feedbacks in the Nd–LWP system, a weaker negative Nd–LWP relationship is observed over most of the globe. This relationship is highly sensitive to the initial cloud state, illuminating the roles of different processes in shaping the Nd–LWP relationship. The nature of the current observing system limits this work to a single time period for observations, highlighting the need for more frequent observations of key cloud properties to constrain cloud behaviour at process timescales.

Abstract. The effects of aerosols on cloud microphysical properties are a large source of uncertainty when assessing anthropogenic climate change. The aerosol–cloud relationship is particularly unclear in high-latitude polar regions due to a limited number of observations. Cloud liquid water path (LWP) is an important control on cloud radiative properties, particularly in the Arctic, where clouds play a central role in the surface energy budget. Therefore, understanding how aerosols may alter cloud LWP is important, especially as aerosol sources such as industry and shipping move further north in a warming Arctic. Using satellite data, this work investigates the effects of aerosols on liquid Arctic clouds over open ocean by considering the relationship between cloud droplet number concentration (Nd) and LWP, an important component of the aerosol–LWP relationship. The LWP response to Nd varies significantly across the region, with increases in LWP with Nd observed at very high latitudes in multiple satellite datasets, with this positive signal observed most strongly during the summer months. This result is in contrast to the negative response typically seen in global satellite studies and previous work on Arctic clouds showing little LWP response to aerosols. The lower tropospheric stability (LTS) was found to be an important control on the spatial variations in LWP response, strongly influencing the sign and magnitude of the Nd–LWP relationship, with increases in LWP in high-stability environments. The influence of humidity varied depending on the stability, with little impact at low LTS but a strong influence at high LTS. The mean Nd state does not dominate the LWP response, despite the non-linearities in the relationship. As the Nd–LWP sensitivity changed from positive to negative when moving from high- to low-LTS environments, this work shows evidence of a temperature-dependent aerosol indirect effect. Additionally, the LWP–LTS relationship changes with Nd, generating an aerosol-dependent cloud feedback. As the LTS is projected to decrease and the boundary layer to become more polluted in a future Arctic, these results show that aerosol increases may produce lower cloud water paths. This shift to more unstable environments implies that LWP adjustments shift from enhancing the Twomey effect by 8 % to offsetting it by around 40 %, with this warming effect having potential consequences for sea ice extent.

Cu-C6F5]4 is a thermally stable and soluble compound with suitable reactivity for synthetic applications in organic and inorganic chemistry. Here the synthesis of [Cu-C6F5]4 is explored in different solvents and followed by in-situ 19 F NMR spectroscopy. The importance of solvent choice during the synthesis from Grignard reagent C6F5MgBr is highlighted, with a range of magnesium cuprate species identified and isolated when THF is used as solvent (rather than Et2O), including [Cu(C6F5)2]and the remarkable organocopper polyanion ([Cu5(C6F5)7] 2-)∞. The coordination chemistry of [Cu-C6F5]4 with 1,4-dioxane is investigated in solution and in the solid state, with an extended coordination network, [Cu-C6F5]4(dioxane), structurally resolved for the first time. This structure reveals interwoven linear and zig-zag chains featuring dioxane donors unusually coordinating to adjacent Cu sites of some of the [Cu-C6F5]4 tetramers.

Abstract. The aerosol impact on liquid water path (LWP) is a key uncertainty in the overall climate impact of aerosol. However, despite a significant effort in this area, the size of the effect remains poorly constrained, and even the sign is unclear. Recent studies have shown that the relationship between droplet number concentration (Nd) and LWP is an unreliable measure of the impact of Nd variations on LWP due to the difficulty in establishing causality. In this work, we use satellite observations of the short-term development of clouds to examine the role of Nd perturbations in LWP variations. Similar to previous studies, a increase followed by a general decrease in LWP with increasing Nd is observed, suggesting an overall negative LWP response to Nd and a warming LWP adjustment to aerosol. However, the Nd also responds to the local environment, with aerosol production, entrainment from the free troposphere and wet scavenging all acting to modify the Nd. Many of these effects act to further steepen the Nd-LWP relationship and obscure the causal Nd impact on LWP. Using the temporal development of clouds to account for these feedbacks in the Nd-LWP system, a weaker negative Nd-LWP relationship is observed over most of the globe. This relationship is highly sensitive to the initial cloud state, illuminating the roles of different processes in shaping the Nd-LWP relationship. The nature of the current observing system limits this work to a single timeperiod for observations, highlighting the need for more frequent observations of key cloud properties to constrain cloud behaviour at process timescales.

No abstract